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The homochirality of biomolecules remains one of the outstanding puzzlesconcerning the beginning of life. Chiral amplification of a randomly perturbedracemic mixture of chiral molecules is a well-accepted prerequisite for allroutes to biological homochirality. Some models have suggested that suchamplification occurred due to asymmetric discrimination of chiral biotic orprebiotic molecules when they adsorbed onto crystalline surfaces. While chiralamplification has been demonstrated on surfaces of both chiral and achiralcrystals, the mechanism that would produce an enantiomeric imbalance in thechiral surfaces themselves has not been addressed. Here we report strong chiralamplification in the colloidal synthesis of intrinsically chiral lanthanidephosphate nanocrystals, quantitatively measured via the circularly polarizedluminescence of the lanthanide ions within the nanocrystals. The amplificationinvolves spontaneous symmetry breaking into either left- or right-handednanocrystals below a critical temperature. Furthermore, chiral tartaric acidmolecules in the solution act as an external chiral field, sensitivelydirecting the amplified nanocrystal handedness through a discontinuoustransition between left- and right-handed excess. These characteristics suggesta conceptual framework for chiral amplification, based on the statisticalthermodynamics of critical phenomena, which we use to quantitatively accountfor the observations. Our results demonstrate how chiral minerals with highenantiomeric excess could have grown locally in a primordial racemic aqueousenvironment.

Spontaneous and Directed Symmetry Breaking in the Formation of Chiral Nanocrystals